Terahertz Pulses Research Articles

Frequency response of terahertz electro-optic sampling detection technology with thin GaSe crystal

GaSe crystal has good applications in the broadband terahertz pulse generation and electro-optic sampling detection technology. In this paper, the frequency responses of GaSe crystal with different thicknesses in the electro-optic sampling (EOS) detection technology are investigated based on the numerical calculations. Then, the pulse distortions of terahertz induced by the EOS detection technology with thin GaSe crystal are investigated. It is found that the lower the central frequency of the terahertz pulse is, the less the distortion is. When the central frequency of terahertz pulse is higher than 4 THz, the pulse distortions, including the frequency shift and the bandwidth changing, are greatly obvious. Both induced by the EOS technology with different thickness of GaSe crystal are also given in detail. This work provides a good reference to evaluate the performance of EOS detection technology with thin GaSe crystal in the broadband terahertz science and technology.

Gate-readout and a 3D rectification effect for giant responsivity enhancement of asymmetric dual-grating-gate plasmonic terahertz detectors

Abstract We experimentally investigated the asymmetric dual-grating-gate plasmonic terahertz (THz) detector based on an InGaAs-channel high-electron-mobility transistor (HEMT) in the gate-readout configuration. Throughout the THz pulse detection measurement on the fabricated device, we discovered a new detection mechanism called the “3D rectification effect” at the positive gate bias application, which is a cooperative effect of the plasmonic nonlinearities in the channel with the diode nonlinearity in the heterobarrier between the InGaAs channel layer and the InAlAs spacer/carrier-supply/barrier layers, resulting in a giant enhancement of the detector responsivity. We also found that an undesired long-tail waveform observed on the temporal pulse photoresponse of the device is due to trapping of carriers to the donor levels in the silicon δ-doped carrier-supply layer when they tunnel through the barrier to the gate and can be eliminated completely by introducing the so-called inverted-HEMT structure. The internal current responsivity and noise-equivalent power are estimated to be 0.49 A/W (with the equivalent voltage responsivity of 4.9 kV/W with a high output impedance of 10 kΩ) and 196 pW/√Hz at 0.8 THz. These results pave the way towards the application of the plasmonic THz detectors to beyond-5G THz wireless communication systems.

Femtosecond Laser-Induced Emission of Coherent Terahertz Pulses from Ruthenium Thin Films.

We demonstrate emission of electromagnetic pulses with frequencies in the terahertz (THz) range from ruthenium thin films through a second-order nonlinear optical process. Ruthenium deposited on different substrates showed different THz emission properties. We provide evidence that for Ru on glass above a certain power threshold, laser-induced oxidation occurs, resulting in an increased slope of the linear dependence of the THz electric field amplitude on pump power. The THz electric field is mainly polarized parallel to the sample surface, pointing in the same direction everywhere. In contrast to Ru on glass, the electric field amplitude of the THz pulses emitted by Ru on sapphire and on CaF2 shows a simple single linear dependence on pump power, and it is polarized orthogonal to the sample surface. In this case, thermal oxidation in an oven enhances the emission and introduces an additional polarization component along the sample surface. This component also points in the same direction everywhere on the surface, similar to the as-deposited Ru on glass. Although the precise THz generation mechanism remains an open question, our results show a strong correlation between the emission strength and the degree of oxidation. Furthermore, the results highlight the importance of the interfaces, i.e., both the choice of the substrate and the chemical composition of the top surface in THz emission experiments. Knowledge of the state of the sample surface is therefore crucial for the interpretation of THz emission experiments from (nonmagnetic) metal surfaces.

Terahertz radiation from shockwave front irradiated with femtosecond optical pulses

AbstractFemtosecond double optical pulse experiments with nanosecond time delay were conducted in air. Terahertz pulses were generated from laser plasmas produced by the irradiation with the main pulses on shockwave excited by the pre‐pulse illumination. Intensity of the terahertz pulses depends on the time difference Δt and relative position Δy between the pre‐ and main pulses. We found a characteristic dependence of the intensity of the terahertz pulses on Δy at a longer time delay, Δt = 14.7 ns, which has two maxima while only one maximum was observed when delay times were at and shorter than 9.7 ns. The results are discussed taking into account air density distribution of the shockwave. The terahertz emission spectroscopy shown here can be a useful technique for investigating density structure and its time variation of shockwave with high temporal resolution.

Nonlinear photocarrier dynamics in multilayer W S e 2 induced by intense terahertz pulses

Non-equilibrium photocarriers in multilayer WSe2 injected by femtosecond laser pulses exhibit extraordinary nonlinear dynamics in the presence of intense THz fields. The THz absorption in optically excited WSe2 rises rapidly in the low THz field regime and gradually ramps up at high intensities. The strong THz pulses drive the photocarriers into sidebands of higher mobility and release trapped charge carriers, which consequently enhance the transient conductivity of WSe2. The spectrally analyzed conductivity reveals distinctive features, indicating that the photocarriers undergo resonant interactions such as carrier-photon scattering.

Tensile loading state sensing and estimation of opaque polymer materials using pulsed-terahertz waves

In this study, we used pulsed terahertz (THz) spectroscopy to analyze the THz optical properties of opaque acrylonitrile–butadiene–styrene (ABS). The phenomenon occurring upon the propagation of pulsed THz waves through ABS was analyzed through measurements of the variations in THz optical parameters (absorption constant, complex dielectric properties, and refractive index). When tensile loading of 0.1–1.5 kN was applied to a specimen, large optical coefficient variations were observed at 0.275, 0.471, and 0.686 THz, regardless of the applied tensile loading. The optical parameter variations were analyzed at 0.275 THz. Moreover, the accuracy of a tensile loading state estimation model established using principal component analysis was analyzed; consequently, random loading was confirmed. The input factor was extracted and calculated, with an error of approximately 3%, except for small loading (100 N).

Ultrafast terahertz spin and orbital transport in magnetic/nonmagnetic multilayer heterostructures and a perspective

Ultrafast optically excited ferromagnetic (FM)/nonmagnetic (NM) multilayer heterostructures have been demonstrated recently as efficient, high-power, and broadband sources of terahertz (THz) electromagnetic radiation. Since these spintronic THz emitters exploit the conversion from ultrafast spin to charge current, either in bulk or at the interface, the THz pulses inhere all the characteristics of the involved mechanisms and dynamics associated with spin-charge interconversion processes. Deconvolving the same requires meticulous and careful experimentation and analysis. In this article, we review the current state-of-the-art in this field and provide a perspective on the emerging phenomena, which are prospering as new research avenues and demonstrate application potential for futuristic THz technologies. In the process of developing efficient spintronic THz emitters by optimizing various conditions including those with material parameters and excitation light, it turns out that THz emission spectroscopy itself can be a unique experimental tool for probing microscopic dynamical magnetic and spintronic effects, induced by femtosecond laser pulse excitation, in a noncontact and noninvasive manner. Several breakthroughs can be listed from the literature in this regard from the last decade. Just recently, ultrafast orbitronics is another dimension that is taking shape and will impact the field immensely. A fair account to this topic is also presented in the article.

Ultrafast snapshots of terahertz electric potentials across ring-shaped quantum barriers

Abstract Probing the time evolution of the terahertz electric field within subwavelength dimensions plays a crucial role in observing the nanoscale lightwave interactions with fundamental excitations in condensed-matter systems and in artificial structures, such as metamaterials. Here, we propose a novel probing method for measuring terahertz electric potentials across nanogaps using a combination of optical and terahertz pulse excitations. To achieve this, we employ ring-shaped nanogaps that enclose a metallic island, allowing us to capture tunneling charges when subjected to terahertz electromagnetic pulse illumination. By controlling and manipulating the terahertz tunneling charges through a focused optical gate pulse, we can obtain the terahertz potential strength as a function of spatial coordinates and time delays between pulses. To accurately quantify the time evolution of terahertz electric potential across quantum barriers, we carefully calibrate the recorded nonlinear tunneling current. Its on-resonance and off-resonance behaviors are also discussed, providing valuable insights into the antenna’s characteristics and performance.

Thickness measurement of polychlorotrifluoroethylene coating over metallic seal using terahertz time-domain spectroscopy

ABSTRACT Polychlorotrifluoroethylene is used as a coating material over metallic seals in low-temperature applications to arrest fluid leakage from the impeller side in turbopumps. Typically, polychlorotrifluoroethylene coating is applied on V-type seals, with a thickness ranging from 80 to 130 μm by spraying an emulsion over the substrate followed by heat treatment. An attempt has been made to measure the polychlorotrifluoroethylene coating thickness over V-type seals using terahertz time-domain spectroscopy in reflection geometry, a noncontact, non-invasive NDT method. When the terahertz pulse from a transmitter photo-conductive antenna is incident on the V-type seal, it penetrates through the polychlorotrifluoroethylene coating. It gets reflected from the coating/base coat interface. Here, the reflected echoes from the air-to-polychlorotrifluoroethylene coating interface and polychlorotrifluoroethylene coating to the basecoat interface get overlapped in the time domain as the polychlorotrifluoroethylene coating layer is very thin. The sparse deconvolution technique separates the individual reflected signals and obtains the time delay signals from various interfaces. From the estimation of time delay values, the thickness of the coating has been computed using the refractive index value extracted using terahertz time-domain spectroscopy in transmission mode before the reflection measurements. The obtained thickness values are in close agreement with the coating thickness measured using optical microscopy.

THz driven field emission: energy and time-of-flight spectra of ions

We present an experimental and numerical study of ion field evaporation from LaB6 nanotips using single-cycle terahertz (THz) transients and a static bias voltage. Varying the amplitude and phase of the THz pulses and the value of the bias, we explore the THz-induced reshaping of the ions energy and their time-of-flight spectra. These results prove that short THz transient of about 1 ps can induce ionization and emission of ions from LaB6 samples by a field effect: the THz transient acts as an ultra-short electrical pulse. Moreover, comparing numerical and experimental results, we prove that the response time of surface atoms to the THz transient is shorter than 1 ps, corresponding to the vibration times of acoustic phonons in LaB6.

Highly sensitive frequency upconversion detection from 1 to 3 THz with OH1 crystal.

The wide applications of terahertz (THz) wave technology in the ∼1-3 THz range has resulted in a surge in the demand for the performance improvement of THz wave detection technique. In this study, a frequency tunable, highly sensitive frequency upconversion detection based on a 2-(3-(4-hydroxystyryl)-5,5-dime-thylcyclohex-2-enylidene) malononitrile (OH1) crystal at room temperature is demonstrated. Moreover, to effectively increase the signal-to-noise ratio in the low frequency range, a beam isolation enhancer is proposed and its effect is verified. The minimum detectable THz pulse energy reaches about 100 aJ at 1.9 THz. The frequency tuning ranging from 1 to 3 THz. Sensitivity comparison with a 4-dimethylamino-N-methyl-4-stilbazolium tosylate (DAST) crystal system shows that OH1 is a more suitable nonlinear crystal in the 1-2.4 THz range.

Generating Angular-Varying Time Delays of THz Pulses via Direct Space-to-Time Mapping of Metasurface Structures.

We experimentally demonstrate the generation of double terahertz (THz) pulses with tailored angular-dependent time delays from a nonlinear metasurface excited by a near-infrared femtosecond pulse. The tailored temporal properties of the generated pulses emerge from a direct mapping of the nonlinear spatial response of the metasurface to the emitted THz temporal profile. We utilize the Pancharatnam-Berry phase to implement symmetric and antisymmetric metasurface configurations and show that the emitted patterns present spatiotemporal "X-shaped" profiles after collimation by a parabolic mirror, with angular-dependent pulse delays corresponding to the intended design. In addition, we show that the addition of polarization multiplexing presents the opportunity to achieve a full range of elliptical THz polarizations. Double pulse generation and spatiotemporal shaping of THz waves in general show potential for THz spectroscopy and molecular dynamics applications, particularly in pump-probe experiments.

Subcycle surface electron emission driven by strong-field terahertz waveforms

The advent of intense terahertz (THz) sources opened a new era when the demonstration of the acceleration and manipulation of free electrons by THz pulses became within reach. THz-field-driven electron emission was predicted to be confined to a single burst due to the single-cycle waveform. Here we demonstrate the confinement of single-cycle THz-waveform-driven electron emission to one of the two half cycles from a solid surface emitter. Either the leading or the trailing half cycle was active, controlled by reversing the field polarity. THz-driven single-burst surface electron emission sources, which do not rely on field-enhancement structures, will impact the development of THz-powered electron acceleration and manipulation devices, all-THz compact electron sources, THz waveguides and telecommunication, THz-field-based measurement techniques and solid-state devices.

Terahertz pulsed imaging of low velocity impact damage in woven fiber composite laminates

Recently, terahertz pulse imaging has been used extensively to characterize internal defects in various electrically insulating materials. In this work, terahertz pulse imaging is used to identify the damage induced by low-velocity impact on woven glass-fiber reinforced polyamide laminates. Several impact energies are considered to study the damage initiation and propagation. The permanent indentation, known to be a relevant damage indicator, is extracted from the terahertz results and validated through comparison with profilometry. Further, the criticality of the damage, in terms of the number of composite plies in which the cracks propagate, can be clearly determined from terahertz imaging. These observations are validated through X-ray tomographic observations and analysis. Finally, a strong connection is established between the evolution of the permanent indentation and the appearance, and criticality, of the low-velocity impact-induced damage. These observations suggest that terahertz imaging is a reliable technique for the nondestructive assessment of impact damage in glass fiber composites.

Terahertz Emission via Optical Rectification in a Metal-Free Perovskite Crystal.

We report on the emission of high-intensity pulsed terahertz radiation from the metal-free halide perovskite single crystal methyl-DABCO ammonium iodide (MDNI) under femtosecond illumination. The power and angular dependence of the THz output implicate optical rectification of the 800 nm pump as the mechanism of THz generation. Further characterization finds that, for certain crystal orientations, the angular dependence of THz emission is modulated by phonon resonances attributable to the motion of the methyl-DABCO moiety. At maximum, the THz emission spectrum of MDNI is free from significant phonon resonances, resulting in THz pulses with a temporal width of <900 fs and a peak-to-peak electric field strength of approximately 0.8 kV cm-1-2 orders of magnitude higher than any other reported halide perovskite emitters. Our results point toward metal-free perovskites as a promising new class of THz emitters that brings to bear many of the advantages enjoyed by other halide perovskite materials. In particular, the broad tunability of optoelectronic properties and ease of fabrication of perovskite materials opens up the possibility of further optimizing the THz emission properties within this material class.

Terahertz radiation by quantum interference of excitons in a one-dimensional Mott insulator

Nearly monocyclic terahertz waves are used for investigating elementary excitations and for controlling electronic states in solids. They are usually generated via second-order optical nonlinearity by injecting a femtosecond laser pulse into a nonlinear optical crystal. In this framework, however, it is difficult to control phase and frequency of terahertz waves. Here, we show that in a one-dimensional Mott insulator of a nickel-bromine chain compound a terahertz wave is generated with high efficiency via strong electron modulations due to quantum interference between odd-parity and even-parity excitons produced by two-color femtosecond pulses. Using this method, one can control all of the phase, frequency, and amplitude of terahertz waves by adjusting the creation-time difference of two excitons with attosecond accuracy. This approach enables to evaluate the phase-relaxation time of excitons under strong electron correlations in Mott insulators. Moreover, phase- and frequency-controlled terahertz pulses are beneficial for coherent electronic-state controls with nearly monocyclic terahertz waves.

Efficient and Continuous Carrier-Envelope Phase Control for Terahertz Lightwave-Driven Scanning Probe Microscopy.

The fundamental understanding of quantum dynamics in advanced materials requires precise characterization at the limit of spatiotemporal resolution. Ultrafast scanning tunneling microscopy is a powerful tool combining the benefits of picosecond time resolution provided by single-cycle terahertz (THz) pulses and atomic spatial resolution of a scanning tunneling microscope (STM). For the selective excitation of localized electronic states, the transient field profile must be tailored to the energetic structure of the system. Here, we present an advanced THz-STM setup combining multi-MHz repetition rates, strong THz near fields, and continuous carrier-envelope phase (CEP) control of the transient waveform. In particular, we employ frustrated total internal reflection as an efficient and cost-effective method for precise CEP control of single-cycle THz pulses with >60% field transmissivity, high pointing stability, and continuous phase shifting of up to 0.75 π in the far and near field. Efficient THz generation and dispersion management enable peak THz voltages at the tip-sample junction exceeding 20 V at 1 MHz and 1 V at 41 MHz. The system comprises two distinct THz generation arms, which facilitate individual pulse shaping and amplitude modulation. This unique feature enables the flexible implementation of various THz pump-probe schemes, thereby facilitating the study of electronic and excitonic excited-state propagation in nanostructures and low-dimensional materials systems. Scalability of the repetition rate up to 41 MHz, combined with a state-of-the-art low-temperature STM, paves the way toward the investigation of dynamical processes in atomic quantum systems at their native length and time scales.

Terahertz Probing of Anisotropic Conductivity and Morphology of CuMnAs Epitaxial Thin Films

AbstractAntiferromagnetic CuMnAs thin films have attracted attention since the discovery of the manipulation of their magnetic structure via electrical, optical, and terahertz pulses, enabling convenient approaches for switching between magnetoresistive states of the film for information storage. However, the magnetic structure and, thus, the efficiency of the manipulation can be affected by the film morphology and growth defects. In this study, the properties of CuMnAs thin films are investigated by probing the asymmetrical growth‐related uniaxial anisotropy of electric conductivity by contact‐free terahertz transmission spectroscopy. It is shown that the terahertz measurements conveniently detect the conductivity anisotropy that is consistent with conventional DC Hall‐bar measurements. Moreover, the terahertz technique allows for considerably finer determination of anisotropy axes, and it is less sensitive to the local film degradation. Thanks to the averaging over a large detection area, the THz probing also allows an analysis of strongly non‐uniform thin films. Using scanning electron and near‐field terahertz microscopies, the observed anisotropic conductivity of CuMnAs is related to the elongation and orientation of growth defects, which both originate in the anisotropic growth of the films. In addition, control over the morphology of defects is demonstrated by using vicinal substrates.

Hidden-information extraction from layered structures through terahertz imaging down to ultralow SNR.

Noninvasive inspection of layered structures has remained a long-standing challenge for time-resolved imaging techniques, where both resolution and contrast are compromised by prominent signal attenuation, interlayer reflections, and dispersion. Our method based on terahertz (THz) time-domain spectroscopy overcomes these limitations by offering fine resolution and a broadband spectrum to efficiently extract hidden structural and content information from layered structures. We exploit local symmetrical characteristics of reflected THz pulses to determine the location of each layer, and apply a statistical process in the spatiotemporal domain to enhance the image contrast. Its superior performance is evidenced by the extraction of alphabetic characters in 26-layer subwavelength papers as well as layer reconstruction and debonding inspection in the conservation of Terra-Cotta Warriors. Our method enables accurate structure reconstruction and high-contrast imaging of layered structures at ultralow signal-to-noise ratio, which holds great potential for internal inspection of cultural artifacts, electronic components, coatings, and composites with dozens of submillimeter layers.

Calibration of terahertz sampling detectors for intense unipolar picosecond current pulses in waveguides

Terahertz pulses are nowadays commonly used in many areas of condensed matter physics to access material properties and explore transport phenomena at fast timescales. However, little work has been devoted to the full characterization of such pulses when confined in waveguides. In this work, we fabricate terahertz photoconductive switch detectors, located at various points along a coplanar waveguide, and sample the electrical pulses that pass by the detectors. Two different but consistent methods were developed to calibrate the pulse amplitude. Notably, we synchronize a commercial pulse generator with the laser in order to sample nanosecond-wide pulses with the photoswitch detectors, effectively turning the setup into an on-chip high-frequency sampling oscilloscope. Both methods give identical results on pulse current, voltage, and field amplitudes and enable an absolute characterization of the electrical pulse propagation along the waveguide. These techniques constitute a reliable tool to explore (non-linear) phenomena such as current or field induced magnetization switching or phase transitions, which take place at high THz intensities.